贵金属硫化物低电子态激光诱导荧光光谱研究

项目名称： 贵金属硫化物低电子态激光诱导荧光光谱研究

项目编号： No.11274316

项目类型： 面上项目

立项/批准年度： 2013

项目学科： 数理科学和化学

项目作者： 杨杰

作者单位： 中国科学院近代物理研究所

项目金额： 93万元

中文摘要： 贵金属硫化物分子（贵金属原子Ru~Ag/Os~Au结合含硫基团-S/-SH）在地质矿产、合成、催化和生物科学等领域有着广泛的应用前景。然而，直到目前对于贵金属硫化物电子态结构的谱学研究工作非常稀少，极大的限制了对其电子态结构的理解以及潜在的可能应用的认识。本申请，结合激光溅射和超声射流分子束脉冲放电装置（DALAS源），产生贵金属硫化物气相分子，利用新建成的高灵敏、高分辨的激光诱导荧光光谱（LIF）实验装置，研究其电子基态和低能量激发态结构。实验精确测量贵金属硫化物的振动/转动分辨的紫外-可见光谱，通过光谱分析，确定各电子态的对称性，获得分子在不同电子态的转动常数、振动频率等光谱常数，键长、键角等几何构型，电子态中自旋轨道耦合等各种相互作用的类型及强度等，给出分子电子态势能面特征的信息。结合并对比量子化学计算结果，进一步加深对贵金属硫化物低电子态结构的理解。

中文关键词： 贵金属硫化物；自由基；电子态；氧化铜分子；氧化金分子

英文摘要： It is well known that the noble metal sulfides and hydrosulfides are widely used in mineral, synthesis, catalysis, fuel cell and biological sciences. However, among all of the noble metal sulfides, only AuS and AuS2 molecules have been experimentally studied in the gas phase by the photoelectron spectroscopy (PES). The few experimental works greatly limited the understanding of the electronic structures and their potential applications. The development of the new techniques, such as high-resolution laser, supersonic molecule beam, laser ablation and laser induced fluorescence (LIF), had made it possible to study those unstable molecules, including the free radicals. Experimentally, the noble metal sulfides and hydrosulfides molecules can be created by the DALAS source, which combines supersonic molecule beam jet, laser ablation and high voltage pulsed discharge. The newly invented SYNC-LIF technology will be used to identify the desired molecular fluorescence from noisy emission background of variuos particals which are generated during laser ablation and discharge processes. High-resolution LIF spectroscopy will study the electronic transitions among the low-energy electronic states, and provide detailed spectroscopic information which plays important role in understanding how the 4d/5d electrons of transition

英文关键词： noble metal sulfide；free radical；electronic state；CuO molcule；AuO molecule